Angewandte Chemie, Accepted Article.
Two‐dimensional (2D) mesoporous heterostructures combining ultrathin nanosheet morphology, periodic porous surface structures and diverse hybrid compositions have recently emerged and become increasingly important for renewable energy storage and electronics. However, it remains a great challenge to develop a universal method to prepare 2D mesoporous heterostructures. Here, we report a composite micelle‐directed interfacial assembly method to synthesize vertical heterostructures with ultrathin 2D material and two surrounding mesoporous monolayers assembled on both sides. To demonstrate the concept, we first fabricate a new sandwich‐like carbon@MXene@carbon mesoporous heterostructure through self‐assembly of MXene nanosheets and block copolymer F127/melamine‐formaldehyde resin composite micelles as well as a subsequent thermal treatment. We also show that this approach can be applied to other 2D materials (for example, graphene oxide, potassium niobate nanosheets, and zeolitic imidazolate frameworks. Finally, we demonstrate that the carbon@MXene@carbon mesoporous heterostructured nanosheets manifest remarkably enhanced electrochemical performance as cathode for lithium sulfur batteries.